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arXiv:1109.6895 · Optics Express

Quantum-correlated two-photon transitions to excitons in semiconductor quantum wells

Luis J. Salazar, David Guzmán, Ferney J. Rodríguez, Luis Quiroga

Published Feb 8, 2012• 13 citations
arXivHTMLPDF

Abstract

The dependence of the excitonic two-photon absorption on the quantum correlations (entanglement) of exciting biphotons by a semiconductor quantum well is studied. We show that entangled photon absorption can display very unusual features depending on space-time-polarization biphoton parameters and absorber density of states for both bound exciton states as well as for unbound electron-hole pairs. We report on the connection between biphoton entanglement, as quantified by the Schmidt number, and absorption by a semiconductor quantum well. Comparison between frequency-anti-correlated, unentangled and frequency-correlated biphoton absorption is addressed. We found that exciton oscillator strengths are highly increased when photons arrive almost simultaneously in an entangled state. Two-photon-absorption becomes a highly sensitive probe of photon quantum correlations when narrow semiconductor quantum wells are used as two-photon absorbers.

DOI
10.1364/oe.20.004470

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The dependence of the excitonic two-photon absorption on the quantum correlations (entanglement) of exciting biphotons by a semiconductor quantum well is studied. We show that entangled photon absorption can display very unusual features depending on space-time-polarization biphoton parameters and absorber density of states for both bound exciton states as well as for unbound electron-hole pairs. We report on the connection between biphoton entanglement, as quantified by the Schmidt number, and absorption by a semiconductor quantum well. Comparison between frequency-anti-correlated, unentangled and frequency-correlated biphoton absorption is addressed. We found that exciton oscillator strengths are highly increased when photons arrive almost simultaneously in an entangled state. Two-photon-absorption becomes a highly sensitive probe of photon quantum correlations when narrow semiconductor quantum wells are used as two-photon absorbers.
Two-photon absorption spectroscopy was performed in GaAs quantum wells with photon energy \ensuremath{\Elzxh}\ensuremath{\omega} near half the band gap Eg{\mathrm{E}}_{\mathrm{g}}Eg​. For the case of incident light polarized perpendicular to the confinement direction \ensuremath{\epsilon}^\ensuremath{\perp}z^, the onset of two-photon absorption occurs at the 2P state of the lowest-energy heavy-hole exciton and the absorption increases linearly with 2\ensuremath{\Elzxh}\ensuremath{\omega}-Eg{\mathrm{E}}_{\mathrm{g}}Eg​. For \ensuremath{\epsilon}^\ensuremath{\parallel}z^, the two-photon spectrum is stepped with superpositions of sharp 1S exciton features at odd \ensuremath{\Delta}N light-hole--conduction-band transitions. These results are used to accurately determine exciton binding energy, successive subband energy splittings, and band offsets.
Exciton-biexciton coherent coupling effects are examined in semiconductor quantum dots. The exciton absorption spectrum is measured with the microphotoluminescence excitation technique in a single InGaAs quantum dot. The spectrum changes from a Lorenztian-type line shape to an unusual dip-shaped line shape with increasing excitation intensities in a higher exciton state where there is a large oscillator strength between the exciton and biexciton states. The intensity dependence of the dip energy width clearly indicates that coherent Rabi oscillation occurs between the exciton and biexciton states. The absorption properties with excitation light of different polarizations show that the dip-shaped spectra only appear when there is a large biexciton state population with linear polarization. A theoretical analysis undertaken with the density matrix method agrees well with experimental results. This agreement reveals that exciton-biexciton coherent interactions lead to unusual absorption spectra and contribute crucially to the optical properties of quantum dots. The exciton-biexciton coherent effects provide a scheme for controlling four distinguishable states, which can be applied to a demonstration of quantum gate operations.
We propose a three-pulse coherent ultrafast optical technique that is particularly sensitive to two-exciton correlations. Two Liouville-space pathways for the density matrix contribute to this signal which reveals double quantum coherences when displayed as a two-dimensional correlation plot. Two-exciton couplings spread the cross peaks along both axes, creating a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo, in which two-exciton couplings show up along a single axis and are highly congested.
Nonlinear spectroscopic techniques using entangled photon pairs can provide an opportunity to exploit non-classical correlations encoded in two-photon wavefunctions to manipulate two-exciton wavefunctions. We propose an entangled photon pair-enhanced multidimensional spectroscopic technique that is sensitive to exciton-exciton interactions and correlations at the femtosecond timescale. Simulations for a dissipative system, namely, the photosynthetic aggregate reveal the superior ability of entangled photon pairs, compared to both transform-limited and frequency-chirped laser pulses, to manipulate excited-state absorption pathways. The corresponding spectral features in the two-dimensional spectrogram are interpreted in terms of one- and two-exciton resonances. The signal scales linearly with the incoming intensity of the photon sources. We show that classifying these resonances using entangled photon source in the perturbative limit allow for probing exciton correlations at the natural energy scale. These insights can be used to explore multi-exciton dynamics in molecular systems using multiphoton entanglement.
We study photons entangling in the short-time response of a quantum well excited by a short intense pulse. At the time scales, where the biexciton effect is not yet pronounced, the Pauli principle is responsible for many-body correlations among excitons, giving rise to the production of entangled photons with a yield $\ensuremath{\sim}{10}^{\ensuremath{-}2}$. The quantum-field theoretical two-particle density matrix in second quantization is used to calculate the entanglement for arbitrary emission angles of the entangled pairs of photons. At the time scales, where the heavy-light hole splitting is resolved, the resonances corresponding to different two-exciton states develop, which allow for a simple kinematic theory relating the states of the outgoing photons with the respective two-exciton states. The resonant response can be expected at symmetric emission angles for resonances with the heavy-heavy and light-light two-exciton states with remarkably nontrivial dependence of entanglement on the emission angles and on the ellipticity parameters of the excitation. We show that the emitted entangled two-photon states are always in a triplet state.